Discovery of a Wurtzite-like Cu2FeSnSe4 Semiconductor Nanocrystal Polymorph and Implications for Related CuFeSe2 Materials

Tappan, Bryce A.; Chu, Weibin; Mecklenburg, Matthew; Prezhdo, Oleg V.; Brutchey, Richard L.

doi:10.1021/acsnano.1c03974

Title: Discovery of a Wurtzite-like Cu₂FeSnSe₄ Semiconductor Nanocrystal Polymorph and Implications for Related CuFeSe₂ Materials

Journal Article · Wed Aug 04 00:00:00 EDT 2021 · ACS Nano

DOI:https://doi.org/10.1021/acsnano.1c03974· OSTI ID:1866258

Tappan, Bryce A. ^[1];

^[1];

^[1]

Univ. of Southern California, Los Angeles, CA (United States)

I₂-II-IV-VI₄ and I-III-VI₂ semiconductor nanocrystals have found applications in photovoltaics and other optoelectronic technologies because of their low toxicity and efficient light absorption into the near-infrared. Herein, we report the discovery of a metastable wurtzite-like polymorph of Cu₂FeSnSe₄, a member of the I₂-II-IV-VI₄ family of semi-conductors containing only Earth-abundant metals. Density functional theory calculations on this metastable poly-morph of Cu₂FeSnSe₄ indicate that it may be a superior semiconductor for solar energy and optoelectronics applications compared to the thermodynamically preferred stannite polymorph, since the former displays a sharper dispersion of energy levels near the conduction band minimum that can enhance electron mobility and suppress hot electron cooling. The experimental optical band gap was measured by the inverse logarithmic derivative method to be direct, in agreement with theory, and in the range of 1.48-1.59 eV. Mechanistic studies reveal that this metastable phase de-rives from intermediate Cu₃Se₂ nanocrystals that serve as a structural template for the final hexagonal wurtzite-like product. We compare the chemistry of wurtzite-like Cu₂FeSnSe₄ to the related CuFeSe₂ material system. Our experimental and computational comparisons between Cu₂FeSnSe₄ and CuFeSe₂ help explain both the crystal chemistry of CuFeSe₂ that prevents it from forming wurtzite-like polymorphs and the essential role of Sn in stabilizing the metastable structure of Cu₂FeSnSe₄. Furthermore, this work provides insight into the importance of elemental composition when designing syntheses for metastable materials.

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Research Organization:: Univ. of Southern California, Los Angeles, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0006812; FG02-11ER46826; SC0014429

OSTI ID:: 1866258

Journal Information:: ACS Nano, Vol. 15, Issue 8; ISSN 1936-0851

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
metastable
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nanocrystals
wurtzite
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Title: Discovery of a Wurtzite-like Cu2FeSnSe4 Semiconductor Nanocrystal Polymorph and Implications for Related CuFeSe2 Materials

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Title: Discovery of a Wurtzite-like Cu₂FeSnSe₄ Semiconductor Nanocrystal Polymorph and Implications for Related CuFeSe₂ Materials